Wintertime aerosol chemistry and haze evolution in an extremely polluted city of the North China Plain: significant contribution from coal and biomass combustion

Abstract. The North China Plain (NCP) frequently experiences heavy haze pollution, particularly during wintertime. In winter 2015–2016, the NCP region suffered several extremely severe haze episodes with air pollution red alerts issued in many cities. We have investigated the sources and aerosol evolution processes of the severe pollution episodes in Handan, a typical industrialized city in the NCP region, using real-time measurements from an intensive field campaign during the winter of 2015–2016. The average (±1σ) concentration of submicron aerosol (PM1) during 3 December 2015–5 February 2016 was 187.6 (±137.5) µg m−3, with the hourly maximum reaching 700.8 µg m−3. Organic was the most abundant component, on average accounting for 45 % of total PM1 mass, followed by sulfate (15 %), nitrate (14 %), ammonium (12 %), chloride (9 %) and black carbon (BC, 5 %). Positive matrix factorization (PMF) with the multilinear engine (ME-2) algorithm identified four major organic aerosol (OA) sources, including traffic emissions represented by a hydrocarbon-like OA (HOA, 7 % of total OA), industrial and residential burning of coal represented by a coal combustion OA (CCOA, 29 % of total OA), open and domestic combustion of wood and crop residuals represented by a biomass burning OA (BBOA, 25 % of total OA), and formation of secondary OA (SOA) in the atmosphere represented by an oxygenated OA (OOA, 39 % of total OA). Emissions of primary OA (POA), which together accounted for 61 % of total OA and 27 % of PM1, are a major cause of air pollution during the winter. Our analysis further uncovered that primary emissions from coal combustion and biomass burning together with secondary formation of sulfate (mainly from SO2 emitted by coal combustion) are important driving factors for haze evolution. However, the bulk composition of PM1 showed comparatively small variations between less polluted periods (daily PM2. 5 ≤ 75 µg m−3) and severely polluted periods (daily PM2. 5 > 75 µg m−3), indicating relatively synchronous increases of all aerosol species during haze formation. The case study of a severe haze episode, which lasted 8 days starting with a steady buildup of aerosol pollution followed by a persistently high level of PM1 (326.7–700.8 µg m−3), revealed the significant influence of stagnant meteorological conditions which acerbate air pollution in the Handan region. The haze episode ended with a shift of wind which brought in cleaner air masses from the northwest of Handan and gradually reduced PM1 concentration to < 50 µg m−3 after 12 h. Aqueous-phase reactions under higher relative humidity (RH) were found to significantly promote the production of secondary inorganic species (especially sulfate) but showed little influence on SOA.